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Register a new userMid-infrared laser phase-locking to a remote near-infrared frequency reference for high precision molecular spectroscopy
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Authors
Bruno Chanteau
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We present a new method for accurate mid-infrared frequency measurements and stabilization to a near-infrared ultra-stable frequency reference, transmitted with a long-distance fibre link and continuously monitored against state-of-the-art atomic fountain clocks. As a first application, we measure the frequency of an OsO4 rovibrational molecular line around 10 $mu$m with a state-of-the-art uncertainty of 8x10-13. We also demonstrate the frequency stabilization of a mid-infrared laser with fractional stability better than 4x10-14 at 1 s averaging time and a line-width below 17 Hz. This new stabilization scheme gives us the ability to transfer frequency stability in the range of 10-15 or even better, currently accessible in the near-infrared or in the visible, to mid-infrared lasers in a wide frequency range.
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We report the coherent phase-locking of a quantum cascade laser (QCL) at 10-$mu$m to the secondary frequency standard of this spectral region, a CO2 laser stabilized on a saturated absorption line of OsO4. The stability and accuracy of the standard are transferred to the QCL resulting in a line width of the order of 10 Hz, and leading to our knowledge to the narrowest QCL to date. The locked QCL is then used to perform absorption spectroscopy spanning 6 GHz of NH3 and methyltrioxorhenium, two species of interest for applications in precision measurements.
Dual-comb spectroscopy has been proven a powerful tool in molecular characterization, which remains challenging to implement in the mid-infrared (MIR) region due to difficulties in the realization of two mutually locked comb sources and efficient photodetection. An effective way to overcome those limitations is optical upconversion; however, previously reported configurations are either demanding or inefficient. Here we introduce and experimentally demonstrate a variant of dual-comb spectroscopy called cross-comb spectroscopy, in which a MIR comb is upconverted via sum-frequency generation (SFG) with a near-infrared (NIR) comb with a shifted repetition rate and then interfered with a spectral extension of the NIR comb. We experimentally demonstrate a proof-of-concept measurement of atmospheric CO2 around 4.25 micrometer, with a 350-nm instantaneous bandwidth and 25000 resolved comb lines. Cross-comb spectroscopy can be realized using up- or down-conversion and offers an adaptable and efficient alternative to dual-comb spectroscopy outside the well-developed near-IR region, where having two mutually coherent sources and efficient photodetection is challenging. Moreover, the nonlinear gating in cross-comb spectroscopy promises a superior dynamic range compared to dual-comb spectroscopy.
Injection locking is a well known and commonly used method for coherent light amplification. Usually injection locking is done with a single-frequency seeding beam. In this work we show that injection locking may also be achieved in the case of multi-frequency seeding beam when slave laser provides sufficient frequency filtering. One relevant parameter turns out to be the frequency detuning between the free running slave laser and each injected frequency component. Stable selective locking to a set of three components separated of $1.2,$GHz is obtained for (positive) detuning values between zero and $1.5,$GHz depending on seeding power (ranging from 10 to 150 microwatt). This result suggests that, using distinct slave lasers for each line, a set of mutually coherent narrow-linewidth high-power radiation modes can be obtained.
We discuss the laser frequency comb as a near infrared astronomical wavelength reference, and describe progress towards a near infrared laser frequency comb at the National Institute of Standards and Technology and at the University of Colorado where we are operating a laser frequency comb suitable for use with a high resolution H band astronomical spectrograph.
Frequency combs have revolutionized time and frequency metrology and in recent years, new frequency comb lasers that are highly compact or even on-chip have been demonstrated in the mid-infrared and THz regions of the electromagnetic spectrum. The emerging technologies include electrically pumped quantum and interband cascade semiconductor devices, as well as high-quality factor microresonators. In this guest editorial, the authors summarize recent advances in the field, the potential for rapid broadband spectroscopy, as well as the challenges and prospects for use in molecular gas sensing.
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